Non-uniformities in miscible surfactant-laden two-layer thin liquid films

Thin liquid films play an instrumental role in the coating industry. In many cases, these films consist of multiple components and are applied in multiple layers. However, multilayer multicomponent coatings can readily develop thickness non-uniformities due to Marangoni flows driven by solute concentration gradients. Previous flow visualisation experiments have demonstrated that the addition of surfactant can suppress such non-uniformities, but the physical mechanisms underlying this suppression have not yet been definitively established. We investigate the growth of film-height non-uniformities in a two-layer multicomponent coating consisting of a solute-rich bottom layer, a solute-depleted top layer and surfactant. A lubrication-theory-based model that accounts for vertical and lateral gradients in solute and surfactant concentrations is developed. The resulting coupled nonlinear partial differential equations describing the film height, solute concentration and surfactant concentration are solved with a pseudospectral method. Our findings reveal that surfactant-induced Marangoni flows can significantly decrease film-height non-uniformities by competing with Marangoni flows due to solute concentration gradients. Several simplifications of the governing equations are explored to determine how well predictions from these simplified models compare with the full lubrication-theory-based model, thereby providing insight into dominant physical mechanisms in different parameter regimes. The role of surfactant solubility and sorption kinetics in controlling perturbation growth is also examined.